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Catalysis in Frequency Space : Resolving Hidden Oscillating Minority Phases and Their Catalytic Properties

Knudsen, Jan LU ; Eads, Calley LU orcid ; Klyushin, Alexander LU ; Temperton, Robert LU ; Küst, Ulrike LU orcid ; Boix, Virginia ; Kraina, Azemina LU ; Scardamaglia, Mattia LU ; Shavorskiy, Andrey LU and Kokkonen, Esko LU orcid , et al. (2025) In ACS Catalysis 15(3). p.1655-1662
Abstract

In situ catalysis studies typically correlate catalytic function and majority surface structures, but neglect that difficult-to-detect minority structures might govern catalysis. Here we use an oscillating CO:O2 gas composition to drive structural oscillations on a catalytically active Pd(100) surface and collect X-ray photoelectron spectroscopy data at high measurement frequency to demonstrate that the Fourier-transformed data selectively probe oscillations of minority surface structures and of the gas phase. Using the Fourier transform phase as well as work function shifts in the Fourier-transformed photoemission signal, we synchronize all signals and prove that most CO2 is produced above predominantly CO-covered... (More)

In situ catalysis studies typically correlate catalytic function and majority surface structures, but neglect that difficult-to-detect minority structures might govern catalysis. Here we use an oscillating CO:O2 gas composition to drive structural oscillations on a catalytically active Pd(100) surface and collect X-ray photoelectron spectroscopy data at high measurement frequency to demonstrate that the Fourier-transformed data selectively probe oscillations of minority surface structures and of the gas phase. Using the Fourier transform phase as well as work function shifts in the Fourier-transformed photoemission signal, we synchronize all signals and prove that most CO2 is produced above predominantly CO-covered areas.

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organization
publishing date
type
Contribution to journal
publication status
published
subject
keywords
catalysis, CO oxidation, in situ, operando spectroscopy, Pd(100), time-resolved APXPS
in
ACS Catalysis
volume
15
issue
3
pages
8 pages
publisher
The American Chemical Society (ACS)
external identifiers
  • scopus:85215598736
ISSN
2155-5435
DOI
10.1021/acscatal.4c06355
language
English
LU publication?
yes
additional info
Publisher Copyright: © 2025 The Authors. Published by American Chemical Society.
id
6c04aa7f-cb0f-49fa-ab93-fc3b9e5458ba
date added to LUP
2025-05-05 15:46:02
date last changed
2025-05-06 03:17:38
@article{6c04aa7f-cb0f-49fa-ab93-fc3b9e5458ba,
  abstract     = {{<p>In situ catalysis studies typically correlate catalytic function and majority surface structures, but neglect that difficult-to-detect minority structures might govern catalysis. Here we use an oscillating CO:O<sub>2</sub> gas composition to drive structural oscillations on a catalytically active Pd(100) surface and collect X-ray photoelectron spectroscopy data at high measurement frequency to demonstrate that the Fourier-transformed data selectively probe oscillations of minority surface structures and of the gas phase. Using the Fourier transform phase as well as work function shifts in the Fourier-transformed photoemission signal, we synchronize all signals and prove that most CO<sub>2</sub> is produced above predominantly CO-covered areas.</p>}},
  author       = {{Knudsen, Jan and Eads, Calley and Klyushin, Alexander and Temperton, Robert and Küst, Ulrike and Boix, Virginia and Kraina, Azemina and Scardamaglia, Mattia and Shavorskiy, Andrey and Kokkonen, Esko and Schnadt, Joachim}},
  issn         = {{2155-5435}},
  keywords     = {{catalysis; CO oxidation; in situ; operando spectroscopy; Pd(100); time-resolved APXPS}},
  language     = {{eng}},
  month        = {{02}},
  number       = {{3}},
  pages        = {{1655--1662}},
  publisher    = {{The American Chemical Society (ACS)}},
  series       = {{ACS Catalysis}},
  title        = {{Catalysis in Frequency Space : Resolving Hidden Oscillating Minority Phases and Their Catalytic Properties}},
  url          = {{http://dx.doi.org/10.1021/acscatal.4c06355}},
  doi          = {{10.1021/acscatal.4c06355}},
  volume       = {{15}},
  year         = {{2025}},
}